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Thesis

Spanish

ID: <

http://hdl.handle.net/10251/86211

>

·

DOI: <

10.4995/thesis/10251/86211

>

Where these data come from
Nanomateriales híbridos basados en complejos de metales de transición anclados sobre óxido de grafeno. Aplicaciones catalíticas

Abstract

Graphene-based hybrid materials and transition metal complexes play an important role in the science of materials and catalysis, as well as in other technological fields, as highlighted in the literature. In this doctoral thesis new hybrid nanomaterials based on different transition metal complexes (mono- and multimetallic) anchored on the surface of graphene oxide or graphene oxide modified with organic groups have been developed. This doctoral memory constitutes a "classic" work from the point of view of content structure, which are distributed over seven chapters. In the first chapter, the general considerations and applications of graphene and associated hybrid materials are presented together with a classification of strategies of synthesis and chemical structure of graphene oxides under study. Next, the second chapter addresses the objectives of this research work focused on the study of hybrid nanomaterials based on transition metals and graphene. The third and fourth chapter focuses on the synthesis of delaminated graphene oxide by modifying the conventional Hummers method, which provides the laminar support on which donor oxygen and nitrogen groups are covalently anchored. These groups allow the coordinating or axial immobilization of a chiral Mn (III) -salen complex, to provide hybrid nanocatalysts directed to the enantioselective epoxidation of prochiral alkenes. In the fifth chapter of this specification, the chemical modification of graphene oxide is described by amidation and acylation reactions of the carboxylic groups and by the covalent anchoring of a ruthenium (II) organometallic complex. Hybrid nanomaterials are studied in the catalytic racemization of (S) -1-phenylethanol, and the multifunctional enzyme catalyst (CALB)-Ru-OG in the kinetic resolution of 1- phenylethanol. The sixth chapter focuses on the coordinating immobilization of hexanuclear molybdenum (II) nanoclusters with halogens in graphene oxide to provide nanohybrids that have been investigated in the field of photocatalysis and whose activity has been compared with that obtained under homogeneous conditions. Specifically, photoreduction of H2O to H2 and photooxidation of certain organic substrates has been approached, taking advantage of the photoluminescent properties of the molybdenum (II) clusters and the electronic properties of the graphite materials. The characterization of the molecular complexes and nanomaterials synthesized throughout chapters 3-6 of the present thesis is carried out using chemical and structural analysis techniques and spectroscopic, chromatographic, surface and image techniques. The last chapter, and not the least important, highlights the conclusions obtained in this research. TESIS

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